Data on the chemical composition of water and on amphibian populations were collected at least annually from vernal pool and stream sites in Maryland, Washington, D.C., and Virginia, from 2001 through 2004. The data were collected as part of long-term monitoring projects of the Northeast Region of the Amphibian Research and Monitoring Initiative (ARMI) of the U.S. Geological Survey. Water samples were analyzed for temperature, specific conductance, pH, dissolved-oxygen concentration, acid-neutralizing capacity, and concentrations of total Kjeldahl nitrogen and total phosphorus; in 2004, samples also were analyzed for nitrite plus nitrate concentrations and total nitrogen concentrations. Field and laboratory analytical results of water samples and quality-assurance information are presented. Amphibian population data include the presence of amphibian species and the maximum number of egg masses of wood frogs and spotted salamanders at vernal pools, and counts of amphibians made during stream transect and stream quadrat surveys.